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镍掺杂SiO₂膜的制备及CH₄/CO₂气体分离性能

作者：李文秀李丹丹郑立娇范俊刚张志刚

单位：沈阳化工大学辽宁省化工分离技术重点实验室沈阳　110142

关键词：二氧化硅膜镍掺杂水热稳定性气体分离孔结构

分类号：O613.72

出版年,卷(期):页码：2014,42(3):0416-0

DOI：10.7521/j.issn.0454－5648.2014.03.25

摘要：

以正硅酸乙酯(TEOS)为前驱体，六水合硝酸镍(Ni(NO3)2·6H2O)为镍源，采用溶胶凝胶法制备镍掺杂SiO2膜。研究了水用量及镍含量对镍掺杂SiO2膜的结构及形貌的影响，并对其进行CH4、CO2气体渗透性能测试。结果表明：水酯比为5.5时，制备的10%Ni掺杂SiO2膜具有良好的微孔结构，且孔径约为1.16nm，孔隙率为64.9%。一部分Ni元素以Ni和NiO晶体形式填充于SiO2孔道内，另一部分以Si—O—Ni形式进入SiO2骨架。Ni掺杂SiO2膜在84h内能够保持良好的气体渗透性能，表现出比纯SiO2膜更好的水热稳定性。CH4和CO2的气体渗透通量分别为1.56×107和0.64×107mol/(m2·s·Pa)，CH4/CO2气体分离因子达到2.43。

Ni-doped SiO2 films were prepared by a sol-gel method with tetraethylorthosilicate (TEOS) as a precursor and Ni(NO3)2·6H2O as a nickel source. The effects of water consumption and nickel content on the structure and morphology of the films were investigated, and the CH4/CO2 gas separation performance was analyzed. The results indicate that 10% Ni-doped SiO2 films prepared in a ratio of water to TEOS of 5-5 possess a microporous structure, the pore size is 116nm and the porosity is 64.9%. A certain amount of Ni element in the crystal forms of Ni and NiO was filled into the SiO2 pores, and other amount of Ni element in the form of Si—O—Ni bond was filled into the SiO2 matrix. The Ni-doped SiO2 films have a superior gas permeation in 84h, showing a better hydrothermal stability, compared to the pure SiO2 films. The permeation flux of CH4 and CO2 gas are 1.56×10-7 and 0.64×10-7mol/(m2·s·Pa), respectively, and the CH4/CO2 separation factor is 2.43.

基金项目：

国家自然科学基金(21076126)；辽宁省自然科学基金 (2013020080)资助项目。

作者简介：

第一作者：李文秀(1963－)，男，博士，教授。通信作者：张志刚(1968－)，男，博士，教授。 ———————————— Received date：2013-09-23.　　Revised date：2013-11-27. First author: LI Wenxiu(1963－)，male, Ph.D., Professor. E-mail: wenxli@126.com Corresponding author: ZHANG Zhigang(1968－), male, Ph.D., Professor. E-mail: zhzhgang@126.com

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